Single-layer Graphene Research Articles

Graphene-Based Tunable Dual-Frequency Terahertz Sensor.

A tunable dual-band terahertz sensor based on graphene is proposed. The sensor consists of a metal bottom layer, a middle dielectric layer, and single-layer graphene patterned with four strips on the top. The numerical simulations results show that the proposed sensor exhibits two significant absorption peaks at 2.58 THz and 6.07 THz. The corresponding absorption rates are as high as nearly 100% and 98%, respectively. The corresponding quality factor (Q) value is 11.8 at 2.58 THz and 29.6 at 6.07 THz. By adjusting the external electric field or chemical doping of graphene, the positions of the dual-frequency resonance peak can be dynamically tuned. The excitation of plasma resonance in graphene can illustrate the mechanism of the sensor. To verify the practical application of the device, the terahertz response of different kinds and different thicknesses of the analyte is investigated and analyzed. A phenomenon of obvious frequency shifts of the two resonance peaks can be observed. Therefore, the proposed sensor has great potential applications in terahertz fields, such as material characterization, medical diagnosis, and environmental monitoring.

Self-powered graphene/4H-SiC nanowire array-based ultraviolet photodetectors with fast response time and low dark current for promising wireless ultraviolet communication

Self-powered ultraviolet photodetectors (UV PDs) capable of detecting UV light signals without using an external power supply have become particularly attractive because of their high sensitivity, consistent optical response, ultra-small size, low energy consumption, and long-term robustness for the future. Here we reported a self-powered UV PDs coupling of two-dimensional (2D) single-layer graphene and one-dimensional (1D) 4H-SiC nanowire arrays. The fabricated PDs can feature an ultra-high on-off ratio of 6301 at 0 V and the 2D-1D architectural exhibits a low dark current of ∼4 pA, an ultra-fast response of 4.89 ms. The high performance was associated with the formed heterojunction between the 2D graphene and 1D 4H-SiC nanowire array and the high carrier mobility of the graphene. Moreover, the 2D-1D PDs with a large switching ratio and ultra-fast response time can be beneficial to achieve efficient, real-time, and accurate information transmission under 275 nm UV light, shedding some light on the development of high-performance wireless optical communication systems.

Graphene‐Based Lateral Heterojunctions for 2D Integrated Circuits

AbstractA method for patterning single‐layer graphene (SLG) and single‐layer oxidized graphene (SOG) within a continuous atomic layer to form lateral heterojunctions is presented. Raman spectroscopy is employed to investigate the evolution of defect‐related Raman peaks during excimer‐UV irradiation, facilitating the identification of structural changes and defect formation processes. Electrical transport measurements reveal that SOG‐patterned field‐effect transistors (FETs) exhibit varying characteristics depending on the degree of oxidation, thus offering the potential to tailor the electrical properties of graphene devices for specific requirements. Scanning Kelvin probe microscopy measurements reveal the surface potential and work function of the SOG regions compared with those of SLG. The effective functionality of the SOG pattern to operate as a resistor, allowing control of the electrical conductivity in the SOG‐patterned SLG channels, is demonstrated. This capability restricts the current flow while preserving the pristine electrical properties of the graphene channel. Moreover, the SOG pattern can serve as a potential barrier to constructing SLG‐SOG‐patterned integrated circuits, providing exciting opportunities for engineering advanced electronic components. This breakthrough in graphene devices simplifies the fabrication process of graphene‐based FETs and provides the foundation for developing atomically thin integrated circuits for a wide range of applications.

Single-layer graphene based resistive humidity sensor enhanced by graphene quantum dots

Graphene is broadly applied as sensitive sensing material results from its superb features. Concurrently, as a derivative of graphene with 0D structure, graphene quantum dots (GQDs) offer more possibilities as a supportive sensing material due to its adjustable size and functional group modification. In this work, GQDs are introduced to single-layer graphene (SLG) based humidity sensor to enhance the sensing performance. Specifically, consistent resistance response to relative humidity (RH) is extended from the range of 10%–60% to 10%–90% by contrary to original SLG based sensor. Parallelly, effect of the amount of GQDs is investigated by means of multiple GQDs deposition. As the resultant higher binding efficiency between water molecules and the functional groups of GQDs, improved response rate is observed. For the case of 4-time deposition of GQDs, the response rate ( ΔR/R ) reaches ∼130% in RH range of 10%–90%. Besides, the response time and recovery time are ∼0.7 s and ∼1.1 s, respectively. The fluctuation of the resistance change of the sensor under constant humidity is less than 5% over a month which demonstrates long-term reliability.

Nonlinear wave propagation in graphene incorporating second strain gradient theory

The exploration of graphene has attracted extensive interest owing to its significant structural and mechanical properties. In this research, we numerically investigate wave propagation in defect-free single-layer graphene, considering its geometrically nonlinear behavior through second-strain gradient elasticity. To capture the geometric nonlinearity, firstly, the nonlinear strain–displacement relations are introduced. The governing equation and associated boundary conditions are derived using Hamilton’s principle. Then, the weak form, including the element matrices, is established. The eigenvalue problem is solved for 2D wave propagation through periodic structures theory. Finally, the dynamical properties such as band structures, mode shapes, energy flow, and wave beaming effects are analyzed. The numerical results reveal that the geometric nonlinearity through the second strain gradient influences the wave propagation characteristics in graphene. The findings are significant and contribute to the understanding of graphene’s dynamic response, with implications for the engineering applications of graphene-based nanostructures.

Sequential Bayesian-optimized graphene synthesis by direct solar-thermal chemical vapor deposition

This work reports the use of a high-flux solar simulator that mimics the solar spectrum and a cold-wall CVD reactor to demonstrate the feasibility of utilizing a renewable energy resource in synthesizing graphene under various conditions. A parametric study of process parameters was conducted using a probabilistic approach. Gaussian process regression serves as a surrogate to establish a prior for Bayesian optimization, and an information acquisition function is employed to identify conditions that yield high-quality products. Backscattered electron images and Raman mapping were used to assess the effects of growth conditions on graphene characteristic sizes, film quality, and uniformity. We report the synthesis of high-quality single-layer graphene (SLG) and AB-stacked bilayer graphene films in a one-step, short-time process with ID/IG\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$I_{D}/I_{G}$$\\end{document} ratios of 0.21 and 0.14, respectively. Electron diffraction analysis shows peak intensities that resemble SLG and AB-bilayer graphene with up to 5 and 20 μ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\\upmu }$$\\end{document}m grain sizes, respectively. The optical transmissivities of SLG and AB-bilayer graphene fall between 0.959–0.977 and 0.929–0.953, whereas the sheet resistances measured by a 4-point probe with 1 mm spacing are 15.5 ± 4.6 and 3.4 ± 1.5 kΩ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Omega$$\\end{document}/sq, respectively. Further scale-up of the optimized graphene growth area was achieved by flattening the insolation profile, leading to spatial uniformity up to 13 mm in radius. Direct solar capture for CVD synthesis enable a practical and sustainable option for synthesizing graphene films applicable for photonic and electronic applications.

Electrolyte gated graphene terahertz amplitude modulators

Active manipulation of the amplitude of terahertz (THz) frequency waves, through electrical tuning, is key for next-generation THz imaging and essential for unlocking strategic applications, from wireless communication to quantum technologies. Here, we demonstrate high-performance THz amplitude modulators based on an electrolyte-gated single-layer graphene. Broadband modulation in the 1.5–6 THz range is achieved by optimizing the electric field coupling by carefully controlling the spacer thickness in a quarter-wavelength cavity structure, with a maximum modulation depth of 40% at around 2 THz. Raman characterization confirms a Fermi-level tuning of 0.39 eV via electrolyte gating of graphene. A test 2 × 2 modulator array with independent control of sub-millimeter regions is then developed and tested, with no crosstalk between pixels. The reported results highlight the potential of electrolyte-gated graphene for efficient THz modulation. The single-chip design offers compactness and ease of integration with other electronic components, making it a promising platform for THz spatial light modulators and adaptive optical components.

Measurement of the surface susceptibility of single-layer atomic crystal by the photonic spin Hall effect in momentum space

Fast and robust measurement of the surface susceptibility is still in urgent need for investigation and application of atomically thin crystals. In this work, we propose an effective method to measure the surface susceptibility of single-layer graphene by detecting the photonic spin Hall effect in momentum space. At a graphene interface, the beam separations with different spin states contain an angular component due to the existence of surface susceptibility. By implementing a postselection with real weak value in our scheme, the contribution of the spatial spin-Hall shift is excluded and the angular one is amplified for detection. It is demonstrated that treating the angular shift as a pointer allows for a reliable determination of the surface susceptibility. Our method may pave a way for the optical parameter characterization of two-dimensional atomic crystals via angular metrology.

Tuning Pore Size in Graphene in the Angstrom Regime for Highly Selective Ion-Ion Separation.

Zero-dimensional pores spanning only a few angstroms in size in two-dimensional materials such as graphene are some of the most promising systems for designing ion-ion selective membranes. However, the key challenge in the field is that so far a crack-free macroscopic graphene membrane for ion-ion separation has not been realized. Further, methods to tune the pores in the Å-regime to achieve a large ion-ion selectivity from the graphene pore have not been realized. Herein, we report an Å-scale pore size tuning tool for single layer graphene, which incorporates a high density of ion-ion selective pores between 3.5 and 8.5 Å while minimizing the nonselective pores above 10 Å. These pores impose a strong confinement for ions, which results in extremely high selectivity from centimeter-scale porous graphene between monovalent and bivalent ions and near complete blockage of ions with the hydration diameter, DH, greater than 9.0 Å. The ion diffusion study reveals the presence of an energy barrier corresponding to partial dehydration of ions with the barrier increasing with DH. We observe a reversal of K+/Li+ selectivity at elevated temperature and attribute this to the relative size of the dehydrated ions. These results underscore the promise of porous two-dimensional materials for solute-solute separation when Å-scale pores can be incorporated in a precise manner.

Rapid THz time-of-flight imaging on single layer graphene for conductivity assessment

The assessment of the electrical conductivity of single-layer graphene (SLG) on flexible substrates is pivotal for the advancement of next-generation electronic devices. In this study, we introduce a novel approach utilizing a rapid terahertz time-of-flight (THz-ToF) imaging technique to nondestructively evaluate the conductivity of SLG films transferred onto plastic substrates. Operating at a pixel scan rate of 100 Hz, our method significantly enhances the imaging contrast by exclusively focusing on the surface with SLG, which is demonstrated by a two-fold increase in contrast over continuous wave imaging results. The employment of an iron-doped antenna has been instrumental in obtaining high-fidelity cross-sectional amplitude images of the graphene layers, a feature essential for the inspection of thin and flexible materials. Furthermore, THz-ToF imaging allows us to map the graphene layer even when it is enclosed by an insulating material, enabling the 3D mapping of conductive layers in multilayered structures. We obtained conductivity mapping of SLG on the plastic substrate using Tinkham formula. The superior performance of this method promises a significant leap forward in the rapid and accurate assessment of conductive films, with profound implications for the development of flexible electronics and bendable displays.

ISCOPEM2D V1.0: An In Situ Method to Characterize and Compare Chemical Vapor Deposition Graphene Films Using Quality Matrix Approaches

Single‐layer chemical vapor deposition (CVD) graphene films are commonly transferred from their native growth substrates during characterization. However, the transfer process influences their intrinsic material properties and growth substrate‐related material information is lost. Herein, an in situ method is presented to suspend CVD graphene films directly on their growth substrate. The approach makes the sample compatible for characterization across the widely used optical and electron microscopy techniques such as Raman spectroscopy and transmission electron microscopy. In addition, a quality matrix framework “ISCOPEM2D V1.0” is provided to support the quantification, comparison, and validation of various material properties of single‐layer graphene. The approach provides a holistic overview of various properties and facilitates quality control and reproducibility of single‐layer graphene‐based application development. Similar approaches can be useful to develop quality matrix‐based for other 2D materials.

High-harmonic generation with a twist: all-optical characterization of magic-angle twisted bilayer graphene

If we stack up two layers of graphene while changing their respective orientation by some twisting angle, we end up with a strikingly different system when compared to single-layer graphene. For a very specific value of this twist angle, known as magic angle, twisted bilayer graphene displays a unique phase diagram that cannot be found in other systems. Recently, high-harmonic generation spectroscopy has been successfully applied to elucidate the electronic properties of quantum materials. The purpose of the present work is to exploit the nonlinear optical response of magic-angle twisted bilayer graphene to unveil its electronic properties. We show that the band structure of magic-angle twisted bilayer graphene is imprinted onto its high-harmonic spectrum. Specifically, we observe a drastic decrease of harmonic signal as we approach the magic angle. Our results show that high-harmonic generation can be used as a spectroscopy tool for measuring the twist angle and also the electronic properties of twisted bilayer graphene, paving the way for an all-optical characterization of moiré materials.

On-Site Fluorescent Detection of Sepsis-Inducing Bacteria using a Graphene-Oxide CRISPR-Cas12a (GO-CRISPR) System.

Sepsis is an extremely dangerous medical condition that emanates from the body's response to a pre-existing infection. Early detection of sepsis-inducing bacterial infections can greatly enhance the treatment process and potentially prevent the onset of sepsis. However, current point-of-care (POC) sensors are often complex and costly or lack the ideal sensitivity for effective bacterial detection. Therefore, it is crucial to develop rapid and sensitive biosensors for the on-site detection of sepsis-inducing bacteria. Herein, we developed a graphene oxide CRISPR-Cas12a (GO-CRISPR) biosensor for the detection of sepsis-inducing bacteria in human serum. In this strategy, single-stranded (ssDNA) FAM probes were quenched with single-layer graphene oxide (GO). Target-activated Cas12a trans-cleavage was utilized for the degradation of the ssDNA probes, detaching the short ssDNA probes from GO and recovering the fluorescent signals. Under optimal conditions, we employed our GO-CRISPR system for the detection of Salmonella Typhimurium (S. Typhimurium) with a detection sensitivity of as low as 3 × 103 CFU/mL in human serum, as well as a good detection specificity toward other competing bacteria. In addition, the GO-CRISPR biosensor exhibited excellent sensitivity to the detection of S. Typhimurium in spiked human serum. The GO-CRISPR system offers superior rapidity for the detection of sepsis-inducing bacteria and has the potential to enhance the early detection of bacterial infections in resource-limited settings, expediting the response for patients at risk of sepsis.

Magnetic properties of CoFeB films grown on a single-layer graphene underlayer

Magnetic properties of CoFeB films grown on a single-layer graphene underlayer

A hybrid quantum-classical theory for predicting terahertz charge-transfer plasmons in metal nanoparticles on graphene.

Metal nanoparticle (NP) complexes lying on a single-layer graphene surface are studied with a developed original hybrid quantum-classical theory using the Finite Element Method (FEM) that is computationally cheap. Our theory is based on the motivated assumption that the carrier charge density in the doped graphene does not vary significantly during the plasmon oscillations. Charge transfer plasmon (CTP) frequencies, eigenvectors, quality factors, energy loss in the NPs and in graphene, and the absorption power are aspects that are theoretically studied and numerically calculated. It is shown the CTP frequencies reside in the terahertz range and can be represented as a product of two factors: the Fermi level of graphene and the geometry of the NP complex. The energy losses in the NPs are predicted to be inversely dependent on the radius R of the nanoparticle, while the loss in graphene is proportional to R and the interparticle distance. The CTP quality factors are predicted to be in the range ∼10-100. The absorption power under CTP excitation is proportional to the scalar product of the CTP dipole moment and the external electromagnetic field. The developed theory makes it possible to simulate different properties of CTPs 3-4 orders of magnitude faster compared to the original FEM or the finite-difference time domain method, providing possibilities for predicting the plasmonic properties of very large systems for different applications.

Spin-Selective Memtransistors with Magnetized Graphene.

Spin-polarized bands in pristine and proximity-induced magnetic materials are promising building blocks for future devices. Conceptually new memory, logic, and neuromorphic devices are conceived based on atomically thin magnetic materials and the manipulation of their spin-polarized bands via electrical and optical methods. A critical remaining issue is the direct probe and the optimized use of the magnetic coupling effect in van der Waals heterostructures, which requires further delicate design of atomically thin magnetic materials and devices. Here, a spin-selective memtransistor with magnetized single-layered graphene on a reactive antiferromagnetic material, CrI3, is reported. The spin-dependent hybridization between graphene and CrI3 atomic layers enables the spin-selective bandgap opening in the single-layered graphene and the electric field control of magnetization in a specific CrI3 layer. The microscopic working principle is clarified by the first-principles calculations and theoretical analysis of the transport data. Reliable memtransistor operations (i.e., memory and logic device-combined operations), as well as a spin-selective probe of Landau levels in the magnetized graphene, are achieved by using the subtle manipulation of the magnetic proximity effect via electrical means.

Overview of amorphous carbon memristor device, modeling, and applications for neuromorphic computing

Abstract Carbon-based materials strongly pertain to citizens’ daily life due to their versatile derivatives such as diamond, graphite, fullerenes, carbon nanotube, single-layer graphene, and amorphous carbon (a-C). Compared to other families, a-C exhibits reconfigurable electrical properties by triggering its sp2–sp3 transition and vice versa, which can be readily fabricated by conventional film deposition technologies. For above reasons, a-C has been adopted as a promising memristive material and has given birth to several physical and theoretical prototypes. To further help researchers comprehend the physics behind a-C-based memristors and push forward their development, here we first reviewed the classification of a-C-based materials associated with their respective electrical and thermal properties. Subsequently, several a-C -based memristors with different architectures were presented, followed by their respective memristive principles. We also elucidated the state-of-the-art modeling strategies of a-C memristors, and their practical applications on neuromorphic fields were also described. The possible scenarios to further mitigate the physical performances of a-C memristors were eventually discussed, and their future prospect to rival with other memristors was also envisioned.

Research on electronic and optical properties of pristine and Ag/Au/Cu-doped graphene/MoS2 heterostructures

The Dirac cone in the single-layer graphene limits its application in electronic devices such as Schottky barrier diodes and field-effect transistors. Thus, we make the novel heterostructures based on graphene to solve this problem. The electronic and optical properties of pristine and Ag/Au/Cu-doped graphene/MoS2 heterostructures are investigated by using the density functional theory. For the Ag/Au/Cu-doped MoS2 monolayer, the results show that they are magnetic. Their bands across the Fermi level, which indicates these systems are metallic. For the Ag/Au/Cu-doped graphene/MoS2 heterostructures, they are metallic and nonmagnetic. Especially in the Au-doped graphene/MoS2, the Dirac cone opens about 66 meV. It means that Au-doped graphene/MoS2 has the potential to be a candidate material for high speed electronic devices. Compared with pristine heterostructure, the probability of electron transition in the low energy region is the enhanced in Ag/Au/Cu-doped systems. The optical absorption coefficient of doped heterostructure is enhanced in the range of 0–0.4 eV and 1.7–2.7 eV. This work indicates that these heterostructures have a certain potential in the application of nanodevices.

Machine Learning-Assisted Identification of Single-Layer Graphene via Color Variation Analysis.

Techniques such as using an optical microscope and Raman spectroscopy are common methods for detecting single-layer graphene. Instead of relying on these laborious and expensive methods, we suggest a novel approach inspired by skilled human researchers who can detect single-layer graphene by simply observing color differences between graphene flakes and the background substrate in optical microscope images. This approach implemented the human cognitive process by emulating it through our data extraction process and machine learning algorithm. We obtained approximately 300,000 pixel-level color difference data from 140 graphene flakes from 45 optical microscope images. We utilized the average and standard deviation of the color difference data for each flake for machine learning. As a result, we achieved F1-Scores of over 0.90 and 0.92 in identifying 60 and 50 flakes from green and pink substrate images, respectively. Our machine learning-assisted computing system offers a cost-effective and universal solution for detecting the number of graphene layers in diverse experimental environments, saving both time and resources. We anticipate that this approach can be extended to classify the properties of other 2D materials.

Quantifying defects in graphene oxide structures

Oxidation of graphite and subsequent exfoliation leads to single layer graphene oxide (GO). One of the key structural features of GO is the presence of different kinds of defects that dictates their various physical and chemical properties. Molecular dynamics simulations with ReaxFF force fields have been widely used to generate realistic models of GO. In these simulations, the extent and distribution of the defects are varied by changing the initial oxygen (O)/carbon (C) ratio while the defect density is often measured by the total number of non-graphitic carbon (non-gC) atoms. Our calculations suggest that this parameter overestimates the defect densities at low O/C ratio. Herein, we employ the relative area of the defects as an alternative metric to gauge the defect density. Being exclusive to the defects and sensitive to the structural irregularities, this metric works well at both low and high defect densities. In another example, we consider the reduction of GO to reduced graphene oxide (rGO) for different O/C ratios, where the decrease in the number of non-gC atoms is associated with the formation of comparatively larger defects. Hence, it is unclear whether the extent of reduction in the defect density (if at all) should vary monotonically with the O/C ratio. The defect area, unlike the count of the non-gC atoms, mirrors this ambiguity and the change with respect to O/C ratio is not strictly monotonic. Additionally, we also investigate the dependence of the defect distribution and defect area on the size of the simulation cell.